Ultrafast Electron Correlations and Memory Effects at Work: Femtosecond Demagnetization in Ni

Acharya, Shree Ram; Turkowski, Volodymyr; Zhang, G.  P.; Rahman, Talat S.

doi:10.1103/physrevlett.125.017202

Title: Ultrafast Electron Correlations and Memory Effects at Work: Femtosecond Demagnetization in Ni

Abstract

Experimental observations of the ultrafast (less than 50 fs) demagnetization of Ni have so far defied theoretical explanations particularly since its spin-flipping time is much less than that resulting from spin-orbit and electron-lattice interactions. Through the application of an approach that benefits from spin-flip time-dependent density-functional theory and dynamical mean-field theory, we show that proper inclusion of electron correlations and memory (time dependence of electron-electron interaction) effects leads to demagnetization at the femtosecond scale, in good agreement with experimental observations. Furthermore, our calculations reveal that this ultrafast demagnetization results mainly from spin-flip transitions from occupied to unoccupied orbitals implying a dynamical reduction of exchange splitting. In this work, these conclusions are found to be valid for a wide range of laser pulse amplitudes. They also pave the way for ab initio investigations of ultrafast charge and spin dynamics in a variety of quantum materials in which electron correlations may play a definitive role.

Authors:

^[1]; Turkowski, Volodymyr ^[1];

^[2];

^[1]

Univ. of Central Florida, Orlando, FL (United States)
Indiana State Univ., Terre Haute, IN (United States)

Publication Date:: Tue Jun 30 00:00:00 EDT 2020

Research Org.:: Indiana State Univ., Terre Haute, IN (United States); Univ. of Central Florida, Orlando, FL (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1800368

Grant/Contract Number:: FG02-06ER46304; FG02-07ER46354

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Letters

Additional Journal Information:: Journal Volume: 125; Journal Issue: 1; Journal ID: ISSN 0031-9007

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 74 ATOMIC AND MOLECULAR PHYSICS; Physics

Citation Formats


                    Acharya, Shree Ram, Turkowski, Volodymyr, Zhang, G.  P., and Rahman, Talat S. Ultrafast Electron Correlations and Memory Effects at Work: Femtosecond Demagnetization in Ni.  United States: N. p., 2020. 
Web.  doi:10.1103/physrevlett.125.017202.

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                    Acharya, Shree Ram, Turkowski, Volodymyr, Zhang, G.  P., & Rahman, Talat S. Ultrafast Electron Correlations and Memory Effects at Work: Femtosecond Demagnetization in Ni.  United States.  https://doi.org/10.1103/physrevlett.125.017202

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                    Acharya, Shree Ram, Turkowski, Volodymyr, Zhang, G.  P., and Rahman, Talat S. Tue .  
"Ultrafast Electron Correlations and Memory Effects at Work: Femtosecond Demagnetization in Ni".  United States.  https://doi.org/10.1103/physrevlett.125.017202.  https://www.osti.gov/servlets/purl/1800368.

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@article{osti_1800368,

  title        = {Ultrafast Electron Correlations and Memory Effects at Work: Femtosecond Demagnetization in Ni},

  author       = {Acharya, Shree Ram and Turkowski, Volodymyr and Zhang, G.  P. and Rahman, Talat S.},

  abstractNote = {Experimental observations of the ultrafast (less than 50 fs) demagnetization of Ni have so far defied theoretical explanations particularly since its spin-flipping time is much less than that resulting from spin-orbit and electron-lattice interactions. Through the application of an approach that benefits from spin-flip time-dependent density-functional theory and dynamical mean-field theory, we show that proper inclusion of electron correlations and memory (time dependence of electron-electron interaction) effects leads to demagnetization at the femtosecond scale, in good agreement with experimental observations. Furthermore, our calculations reveal that this ultrafast demagnetization results mainly from spin-flip transitions from occupied to unoccupied orbitals implying a dynamical reduction of exchange splitting. In this work, these conclusions are found to be valid for a wide range of laser pulse amplitudes. They also pave the way for ab initio investigations of ultrafast charge and spin dynamics in a variety of quantum materials in which electron correlations may play a definitive role.},

  doi          = {10.1103/physrevlett.125.017202},

  journal      = {Physical Review Letters},

  number       = 1,

  volume       = 125,

  place        = {United States},

  year         = {Tue Jun 30 00:00:00 EDT 2020},

  month        = {Tue Jun 30 00:00:00 EDT 2020}

}

Copy to clipboard

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Title: Ultrafast Electron Correlations and Memory Effects at Work: Femtosecond Demagnetization in Ni

Abstract

Citation Formats

Magnetization dynamics of Ni and Co films on Cu(001) and of bulk nickel surfaces journal, March 1999

Nonequilibrium Magnetization Dynamics of Nickel journal, June 1997

Ultrafast reduction of exchange splitting in ferromagnetic nickel journal, May 2016

Orbital-selective insulator-metal transition in V 2 O 3 under external pressure journal, January 2006

Ultrafast Spin Dynamics in Ferromagnetic Nickel journal, May 1996

Ultrafast Spin Dynamics of Ferromagnetic Thin Films Observed by fs Spin-Resolved Two-Photon Photoemission journal, December 1997

Femtosecond Electron and Spin Dynamics in N i / W ( 110 ) Films journal, June 2003

Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel journal, March 2018

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Calculation of Coulomb interaction strengths for 3 d transition metals and actinides journal, February 1989

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal, September 2009

Ultrafast and Distinct Spin Dynamics in Magnetic Alloys journal, September 2015

Feedback Effect during Ultrafast Demagnetization Dynamics in Ferromagnets journal, October 2013

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Ultrafast optical manipulation of magnetic order journal, September 2010

Explaining the paradoxical diversity of ultrafast laser-induced demagnetization journal, December 2009

Revealing the Nature of the Ultrafast Magnetic Phase Transition in Ni by Correlating Extreme Ultraviolet Magneto-Optic and Photoemission Spectroscopies journal, August 2018

The spin–flip approach within time-dependent density functional theory: Theory and applications to diradicals journal, March 2003

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Ultrafast Demagnetization Measurements Using Extreme Ultraviolet Light: Comparison of Electronic and Magnetic Contributions journal, January 2012

Electronic structure and effects of dynamical electron correlation in ferromagnetic bcc Fe, fcc Ni, and antiferromagnetic NiO journal, May 2008

Femtosecond modification of electron localization and transfer of angular momentum in nickel journal, August 2007

Role of initial magnetic disorder: A time-dependent ab initio study of ultrafast demagnetization mechanisms journal, June 2019

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Femtosecond Electron and Spin Dynamics in Gd(0001) Studied by Time-Resolved Photoemission and Magneto-optics journal, September 2005

The ultrafast Einstein–de Haas effect journal, January 2019

Ultrafast demagnetization of ferromagnetic transition metals: The role of the Coulomb interaction journal, November 2009

Dynamics of electron-magnon interaction and ultrafast demagnetization in thin iron films journal, November 2008

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Superdiffusive Spin Transport as a Mechanism of Ultrafast Demagnetization journal, July 2010

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Towards TDDFT for Strongly Correlated Materials journal, September 2016

Coherent ultrafast magnetism induced by femtosecond laser pulses journal, May 2009

Self-Consistent Equations Including Exchange and Correlation Effects journal, November 1965

Noncollinear full-potential studies of γ − Fe journal, July 2002

Magnetization dynamics of Ni and Co films on Cu(001) and of bulk nickel surfaces
journal, March 1999

Nonequilibrium Magnetization Dynamics of Nickel
journal, June 1997

Ultrafast reduction of exchange splitting in ferromagnetic nickel
journal, May 2016

Orbital-selective insulator-metal transition in $V_{2} O_{3}$ under external pressure
journal, January 2006

Ultrafast Spin Dynamics in Ferromagnetic Nickel
journal, May 1996

Ultrafast Spin Dynamics of Ferromagnetic Thin Films Observed by fs Spin-Resolved Two-Photon Photoemission
journal, December 1997

Femtosecond Electron and Spin Dynamics in $N i / W (110)$ Films
journal, June 2003

Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel
journal, March 2018

Special points for Brillouin-zone integrations
journal, June 1976

Calculation of Coulomb interaction strengths for 3 d transition metals and actinides
journal, February 1989

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

Ultrafast and Distinct Spin Dynamics in Magnetic Alloys
journal, September 2015

Feedback Effect during Ultrafast Demagnetization Dynamics in Ferromagnets
journal, October 2013

Time-dependent four-component relativistic density functional theory for excitation energies
journal, October 2004

Ultrafast optical manipulation of magnetic order
journal, September 2010

Explaining the paradoxical diversity of ultrafast laser-induced demagnetization
journal, December 2009

Revealing the Nature of the Ultrafast Magnetic Phase Transition in Ni by Correlating Extreme Ultraviolet Magneto-Optic and Photoemission Spectroscopies
journal, August 2018

The spin–flip approach within time-dependent density functional theory: Theory and applications to diradicals
journal, March 2003

Continuous-time Monte Carlo methods for quantum impurity models
journal, May 2011

Inhomogeneous Electron Gas
journal, November 1964

Ultrafast Demagnetization Measurements Using Extreme Ultraviolet Light: Comparison of Electronic and Magnetic Contributions
journal, January 2012

Electronic structure and effects of dynamical electron correlation in ferromagnetic bcc Fe, fcc Ni, and antiferromagnetic NiO
journal, May 2008

Femtosecond modification of electron localization and transfer of angular momentum in nickel
journal, August 2007

Role of initial magnetic disorder: A time-dependent ab initio study of ultrafast demagnetization mechanisms
journal, June 2019

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journal, January 1996

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journal, September 2005

The ultrafast Einstein–de Haas effect
journal, January 2019

Ultrafast demagnetization of ferromagnetic transition metals: The role of the Coulomb interaction
journal, November 2009

Dynamics of electron-magnon interaction and ultrafast demagnetization in thin iron films
journal, November 2008

Local magnetic moments in iron and nickel at ambient and Earth’s core conditions
journal, July 2017

Ultrafast heating as a sufficient stimulus for magnetization reversal in a ferrimagnet
journal, January 2012

Understanding laser-induced ultrafast magnetization in ferromagnets: First-principles investigation
journal, April 2008

Laser-Induced Demagnetization at Ultrashort Time Scales: Predictions of TDDFT
journal, September 2015

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journal, July 2010

Nonadiabatic exchange-correlation kernel for strongly correlated materials
journal, October 2017

Towards TDDFT for Strongly Correlated Materials
journal, September 2016

Coherent ultrafast magnetism induced by femtosecond laser pulses
journal, May 2009

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journal, November 1965

Noncollinear full-potential studies of $γ - Fe$
journal, July 2002